Abstract
AbstractWe report on the largest open‐shell graphenic bilayer and also the first example of triply negatively charged radical π‐dimer. Upon three‐electron reduction, bilayer nanographene fragment molecule (C96H24Ar6)2 (Ar=2,6‐dimethylphenyl) (12) was transformed to a triply negatively charged species 123⋅−, which has been characterized by single‐crystal X‐ray diffraction, electron paramagnetic resonance (EPR) spectroscopy and magnetic properties on a superconducting quantum interference device (SQUID). 123⋅− features a 96‐center‐3‐electron (96c/3e) pancake bond with a doublet ground state, which can be thermally excited to a quartet state. It consists of 34 π‐fused rings with 96 conjugated sp2 carbon atoms. Spin frustration is observed with the frustration parameter f>31.8 at low temperatures in 123⋅−, which indicates graphene upon reduction doping may behave as a quantum spin liquid.
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